Imaging charge transfer in iodomethane upon x-ray photoabsorption

被引：173

作者：

Erk, Benjamin ^{[1
]}

Boll, Rebecca ^{[1
]}

Trippel, Sebastian ^{[2
]}

Anielski, Denis ^{[1
]}

Foucar, Lutz ^{[1
,3
]}

Rudek, Benedikt ^{[1
,4
]}

Epp, Sascha W. ^{[1
]}

Coffee, Ryan ^{[5
]}

Carron, Sebastian ^{[5
]}

Schorb, Sebastian ^{[5
]}

Ferguson, Ken R. ^{[5
]}

Swiggers, Michele ^{[5
]}

Bozek, John D. ^{[5
]}

Simon, Marc ^{[6
]}

Marchenko, Tatiana ^{[6
]}

Kuepper, Jochen ^{[2
,7
]}

Schlichting, Ilme ^{[1
,3
]}

Ullrich, Joachim ^{[1
,4
]}

Bostedt, Christoph ^{[5
]}

Rolles, Daniel ^{[1
,3
]}

Rudenko, Artem ^{[1
,8
]}

机构：

[1] CFEL, Max Planck Adv Study Grp, D-22607 Hamburg, Germany

[2] DESY, Ctr Free Electron Laser Sci CFEL, D-22607 Hamburg, Germany

[3] Max Planck Inst Med Res, D-69120 Heidelberg, Germany

[4] Phys Tech Bundesanstalt, D-38116 Braunschweig, Germany

[5] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA

[6] Univ Paris 06, Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, F-75005 Paris, France

[7] Univ Hamburg, Ctr Ultrafast Imaging, D-22761 Hamburg, Germany

[8] Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA

来源：

SCIENCE | 2014年 / 345卷 / 6194期

基金：

美国国家科学基金会;

关键词：

ELECTRON-TRANSFER; CROSS-SECTIONS; SPECTROSCOPY; COLLISIONS; MOLECULES; DYNAMICS; RATES; IONS;

D O I：

10.1126/science.1253607

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Studies of charge transfer are often hampered by difficulties in determining the charge localization at a given time. Here, we used ultrashort x-ray free-electron laser pulses to image charge rearrangement dynamics within gas-phase iodomethane molecules during dissociation induced by a synchronized near-infrared (NIR) laser pulse. Inner-shell photoionization creates positive charge, which is initially localized on the iodine atom. We map the electron transfer between the methyl and iodine fragments as a function of their interatomic separation set by the NIR-x-ray delay. We observe signatures of electron transfer for distances up to 20 angstroms and show that a realistic estimate of its effective spatial range can be obtained from a classical over-the-barrier model. The presented technique is applicable for spatiotemporal imaging of charge transfer dynamics in a wide range of molecular systems.

引用

页码：288 / 291

页数：4

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